The Dual‐Site Adsorption and High Redox Activity Enabled by Hybrid Organic‐Inorganic Vanadyl Ethylene Glycolate for High‐Rate and Long‐Durability Lithium–Sulfur Batteries

Abstract

Transition metal oxides (TMOs) have attracted considerable attention owing to their strong anchoring ability and natural abundance. However, their single‐site adsorption toward sulfur (S) species significantly lowers the possibility of S species reacting with Li+ in the electrolyte and increases the reaction barrier. This study investigates molecular modification by coupling the TMO structure with Li+ conductive polymer ligands, and vanadyl ethylene glycolate (VEG) is successfully synthesized by introducing organic ligands into the VOx crystal structure. In addition to the strong interaction between the VOx and lithium polysulfides via the V–S bond, the groups in the VEG polymer ligands can reversibly couple/decouple with Li+ in the electrolyte. Such dual‐site adsorption enables a smooth dynamic adsorption‐diffusion process. Accordingly, the VEG‐based Li–S cells exhibit excellent rate reversibility, cyclic stability, and a long cycle life without the addition of conducting agents. Encouragingly, the VEG‐based cells also exhibit close and excellent capacity decays of 0.081%, 0.078%, and 0.095% at 0, 25, and 50 °C (1 C for 200 cycles), respectively. This work provides a novel approach for developing advanced catalysts that can realize Li–S batteries with long‐term durability, fast charge‐discharge properties, and applications in a wide temperature range.

Yttrium-Containing Solid Electrolyte Interphase Safeguards Lithium Anodes in Lithium–Sulfur Batteries

“…Such a film served as a protective layer, guarding the lithium sheet against corrosion and restraining the expansion of lithium dendrites. 37 Furthermore, the decreased area ratio of SO 3 2− /SO 4 2− indicated a decrease in the number of side reactions occurring on the Li anode. In Figure 4e, the Y 3d spectrum displayed peaks at 155.8 eV/157.8 eV, 159.9 eV/ 160.8 eV, and 161.3 eV/161.9 eV, corresponding to different yttrium species, namely yttrium metal, Y−S, and Y−F.…”

“…Y 2 S 3 of the components within the SEI film contributes to the formation of a uniform and compact SEI film. Such a film served as a protective layer, guarding the lithium sheet against corrosion and restraining the expansion of lithium dendrites . Furthermore, the decreased area ratio of SO 3 2– /SO 4 2– indicated a decrease in the number of side reactions occurring on the Li anode.…”

A hierarchical bimetallic nitride hybrid electrode with strong electron interaction for enhanced hydrogen production in seawater

“…30 The bottom layers, about half of the structure, were kept frozen at the lattice position. 31 All structures possessing a dynamic magnetic moment underwent complete relaxation for optimization purposes, without any limitations, until their cumulative energies reached a value below 1 × 10 −6 eV, accompanied by average residual forces below 0.02 eV Å −1 .…”

Theoretical Design of Core–Shell 3d-Metal Nanoclusters for Efficient Hydrogen-Evolving Reaction

“…The spin-polarized calculations were performed starting from default values of NIONS∗1.0 as the initial magnetic moment for each atom in the VASP code . All structures with a dynamic magnetic moment were fully relaxed to optimize without any restriction until their total energies were converged to <10 –6 eV, − and the average residual forces were <0.01 eV/Å . The global transferred charge was calculated by the atomic Bader charge analysis .…”